Enhanced hydrogen-gas permeation through rippled graphene

Wenqi Xiong, Weiqing Zhou, Pengzhan Sun, and Shengjun Yuan
Phys. Rev. B 108, 045408 – Published 17 July 2023
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Abstract

The penetration of atomic hydrogen through defect-free graphene was generally predicted to have a barrier of at least several eV, which is much higher than the 1-eV barrier measured for hydrogen-gas permeation through pristine graphene membranes. Herein, our density functional theory calculations show that ripples, which are ubiquitous in atomically thin crystals and mostly overlooked in the previous simulations, can significantly reduce the barriers for all steps constituting the mechanism of hydrogen-gas permeation through graphene membranes, including dissociation of hydrogen molecules, reconstruction of the dissociated hydrogen atoms and their flipping across graphene. Especially, the flipping barrier of hydrogen atoms from a cluster configuration is found to decrease rapidly down to <1eV with increasing ripples' curvature. The estimated hydrogen permeation rates by fully considering the distribution of ripples with all realistic curvatures and the major reaction steps that occurred on them are quite close to the experimental measurements. Our work provides insights into the fundamental understanding of hydrogen-gas permeation through graphene membranes and emphasizes the importance of nanoscale nonflatness (ripples) in explaining many surface and transport phenomena (for example, functionalization, corrosion and separation) in graphene and other two-dimensional materials.

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  • Received 6 April 2023
  • Revised 5 May 2023
  • Accepted 26 June 2023

DOI:https://doi.org/10.1103/PhysRevB.108.045408

©2023 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Wenqi Xiong1,*, Weiqing Zhou1,*, Pengzhan Sun2,†, and Shengjun Yuan1,3,‡

  • 1Key Laboratory of Artificial Micro- and Nano-structures of the Ministry of Education and School of Physics and Technology, Wuhan University, Wuhan 430072, China
  • 2Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macau 999078, China
  • 3Wuhan Institute of Quantum Technology, Wuhan 430206, China

  • *These authors contributed equally to this work
  • pengzhansun@um.edu.mo
  • s.yuan@whu.edu.cn

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Issue

Vol. 108, Iss. 4 — 15 July 2023

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